Cu-Mn-BTC MOF催化C_(3)H_(6)选择性还原NO的性能  

Performance of Cu-Mn-BTC MOF for selective reduction of NO by propene

作　　者：刘权 苏亚欣[1] 徐国强 温妮妮 周皞 Liu Quan;Su Yaxin;Xu Guoqiang;Wen Nini;Zhou Hao(School of Environmental Science and Engineering,Donghua Unvirsity,Shanghai 201620,China;School of Intelligent Manufacturing,Changzhou Vocational Institute of Engineering,Changzhou 213164,Jiangshu,China)

机构地区：[1]东华大学环境科学与工程学院,上海201620 [2]常州工程技术学院智能制造学院,常州213164

出　　处：《工业催化》2022年第9期21-31,共11页Industrial Catalysis

基　　金：上海市自然科学基金资助项目(19ZR1400700,17ZR1419300);江苏省自然科学基金资助项目(BK20181161);中央高校基本科研业务费项目(2232019D3-24)。

摘　　要：利用丙烯选择性催化还原NO(C_(3)H_(6)-SCR)是具有良好发展前景的脱硝技术之一,但是目前已报道的催化剂存在低温活性较低和氮气选择性不佳等问题。为了研究新型高效的催化剂,通过一步合成法制备了双金属有机骨架材料(x Cu-Mn-BTC MOFs),并研究其在富氧条件下催化C_(3)H_(6)选择性还原NO的脱硝性能。利用SEM、XRD、BET、H_(2)-TPR、XPS和Py-FTIR等技术进行表征,结果表明,Mn的引入显著提高了脱硝效率,其中3.2Cu-Mn-BTC显示出良好的脱硝性能,300℃时NO转化率达80%,N_(2)选择性达94%。SEM和XRD结果表明,Mn成功引入到Cu-BTC骨架中,经过Mn修饰的3.2Cu-Mn-BTC变成了粒径更小的块状晶体;BET结果表明,随着引入Mn含量增加,催化剂比表面积减小,孔径增大;XPS结果表明,3.2Cu-Mn-BTC催化活性较好,与其含有更多吸附氧O_(α)和Cu^(2+)有关;H_(2)-TPR结果表明,与Cu-BTC相比,x Cu-Mn-BTC还原峰向更低温度移动,具有更好的还原能力。Py-FTIR结果表明,经过活化后的x Cu-Mn-BTC催化剂表面含有L酸,Mn的引入增加了催化剂表面L酸性位,L酸是影响C_(3)H_(6)-SCR的重要因素。xCu-Mn-BTC在C_(3)H_(6)-SCR中显示出良好的催化活性,证明双金属MOFs应用于C_(3)H_(6)-SCR的可行性,利用金属的优点合成多金属MOFs来提高C_(3)H_(6)-SCR催化性能可能是未来研究的方向。Selective catalytic reduction of NO with propylene(C_(3)H_(6)-SCR)is a promising denitration technology,but the catalysts reported so far have problems such as low activity at medium and low temperature and poor nitrogen selectivity.In order to develop new and efficient catalysts,a bimetallic organic framework(x Cu-Mn-BTC MOFs)was prepared by a one-step synthesis method,and its performance as a catalyst for reduction of NO with C_(3)H_(6) under excess oxygen was investigated.The relationship between catalyst structure and performance was probed by SEM,BET,XPS,H_(2)-TPR,XRD,Py-FTIR,etc.The results show that the introduction of Mn improves the denitration efficiency.3.2Cu-Mn-BTC shows superior performance,reaching 80%NO conversion and 94%N_(2) selectivity at 300℃.SEM and XRD results show that Mn is successfully introduced into the Cu-BTC framework,and the Mn-modified 3.2Cu-Mn-BTC becomes spherical grains with smaller particle size.BET results show that the specific surface area of the catalyst decreases while the pore diameter increases with an increase of Mn content.XPS result shows that more adsorbed oxygen O_(α) and Cu^(2+)are responsible for the superior catalytic activity of 3.2Cu-Mn-BTC.H_(2)-TPR result shows that compared with Cu-BTC phase,the reduction peak of x Cu-Mn-BTC shifts to a lower temperature,resulting in the better reducing ability.Py-FTIR result shows that the activated x Cu-Mn-BTC catalysts contain Lewis acid.The introduction of Mn increases the Lewis acid sites on the catalyst surface,which is an important factor affecting C_(3)H_(6)-SCR.x Cu-Mn-BTC shows good catalytic activity in C_(3)H_(6)-SCR.The study proves the feasibility of bimetallic MOFs in C_(3)H_(6)-SCR.It is the direction of future research to synthesize multimetallic MOFs by utilizing the advantages of each metal to improve the catalytic performance of C_(3)H_(6)-SCR.

关 键 词：催化化学 选择性催化还原 xCu-Mn-BTC催化剂 NO 丙烯 

分 类 号：TQ426.99[化学工程] O643.36[理学—物理化学] X701[理学—化学]